Process and apparatus for producing photochemical radiations



H. SPINDLER 1,880,333

PROCESS AND APPARATUS FOR PRODUGI-NG PHOTOCHEMIGAL RADIATIONS oct. 4, 1932.A

Filed April 5, 1929 l. .Hwa

Patented Oct. `4, 1932 i HENRY SPINDLER, 0F PARIS, FRANCE f PROCESS AND APPARATUS 'FOB PRDUCING IPHOTOCHEMICAL RADIATIOS Applicationv led April 5, 1929, Serial No. 352,888, and in France April 11, 1928.

The present invention has for its object a n apparatus capable of producing photochemlcal radiations which are very` active and'in particular ultra-violet radiations, notably 5 Schumann, Lyman and Millikan ultra-violet.

As is known, these latter radiations are in resonance with the electronic spheres relatively deep in the atom and thus are capable of producing extremely energetic reactions.

These radiations can be composed of intramolecular transformations of electrochemical polymerizations and condensations of the photolysis, the hydrolysis of the photochemical oxydations. At maximum intensities I l5 can even obtain radio-active reactions.

The apparatus forming the object of the present invention consists essentiallyof a sort of mercury4 vapor furnace, in which the mercury vapor, attaining pressures of several hundred kilograms, is subjected to intensities which are much higher than the intensities utilized up to the present in lamp burners of ordinary mercury.

Said apparatus can comprise forxample a tubular body hermetically closed, in which are disposed electrode tubes filled with mercury and open at their upper part. In the mercury of these electrode tubes plunge tubulatures which terminate each in a chamber forming a burner and in which the are jumps between the levels of mercury of the said electrodes.

The whole can be surrounded by a refrigerating liquid which circulates `at high pressure around the electrode tubes which .form the joint, all variations in pressure within the mercury vapor of the burner being thus transmitted to the outside of the electrode tubes 4 0 in a way to realize a true automatic balancing. The photochemi-cal radiations produced by the umping of the arc in the burner, the tempe'rature of which can attain a value extreme- Y ly high concentrated in a single point, can

i act on the outside ofthe apparatus by means of an aperture furnished with a suitable lens.

f f 5ov l Fig. 1 is a sectional view ithrough the apparatus; y Fig.. 2 is a transverse section onthe line A' A-B of Fig. 1; and

Fig. 3 is a detail in section illustrating the (i5l mercuryjoint or seal. l

Thev apparatus comprises a tubular body 1 ofsteel for example capable of resisting a pressure ofseveral hundred kilograms and surmounted by a chamber 2 closed by means oo of a cover 3 which is tight-litting. 4 is the bottom of the tubular body 1. Itis provided with a joint capable of resisting likewise high v pressures.

On the interior of the tubular body 1 are 6'5 three electrode tubes 5 which traverse the bottom 4 with the interposition of insulators 6, said tubes being closed at their lower extremities by plugs 'Z capable of resisting high pressures and furnished with electrical con- 70 ductors 8. The said electrode tubes are filled with mercury. The li uid refrigerant issuing .from a coil 9 enters y a pipe line 10 into the body of tubular form 1 and leaves the upper chamber'2 by a pipe 11 which brings it 75 back to the coil 9. This liquid refrigerant circulates by reason of the thermo-Siphon effect. The coil 9 housed in a receptacle 12 is fed at 13 with water or other cooling liquid which leaves at 14 the said receptacle 12 and 80 which serves to cool the liquid refrigerant.

The chamber 2 is likewise provided with a branch 15 leading to a manometer 16 and a cock 17 of high pressure type. Finally 18 is a high pressure aperture disposed in the 85 center of the cover 3 of the chamber 2 and furnished with a lens 19 of quartz or fluors or. pIn the mercury of each of the electrode tubes 5- dips a tubulature 20 formed by a tube 90 of quartz open at its lower end (Fig. 3).y These three tubulatures are joined at 21 in a way to constitute a sort of chamber of quartz forming a burner and in which the arc jumps between the levels which the merv cury takes in each of the three electrodes.

The refrigerating liquid which circulates within the assembly composed of tubular body and chamber 2, as stated above, may be water or parailin oil, for example. It thus completely surrounds the part 21 yof the burner in which takes place all the concentration of energy of the apparatus. refrigerant thus is in contact with the upper surface of the mercury of the electrode tubes 5 (see Fig. 3), thereby forming a joint or seal,

in such a way that all variation in pressure internally of the mercur)T vapor` of the burner is transmitted to the outside part of the tubes forming electrodes by the medium of mercury which refills them., A A system of autoequilibration is thus established.

On the inside of chamber 2 and around the burner 21 may be likewise provided a coil 224 for`cooling fed by a pipe 23 with liquid refrigerant leaving by a pipe 24.

Finally I may provide in the walls of the chamber 2 or of the cover 3 all devices for the passage of gas or liquids destined to produce a chemical transformation by means of tions and the like'.

By wayv of a non-limiting example, I will hereinafter indicate how one may proceed with the synthesis of'formaldehyde by means of the photochemical radiations produced by the hereinbefore described apparatus.v For this'purpose I introduce into a tubular system of suitable type subjected to the action of photochemical radiations emanating from thev burner 21 and vtraversing the lens of C5 fcation integrally and containing in addiv 3. Apparatus for the production of photo' quartz or fiuorspar of the aperture 18, a mixture of oxidev of carbons and hydrogen, the

latter gas being in excess with respect to the oxide of carbon in the proportion of about 1: 3 or more. y

I may use for example a mixture as follows: p

y% oxide of ca bon.

`% hydrogen.

Certain known gases, issuing from the gasi- This liquid tion methane, can beutilized for this synthesis.

The tubular system in question in which has been introduced the gaseous mixture is heated to about 300 C. for eliminating all polymerization of the formaldehyde and preventing the formation of other reactions.

There will be more in mixing with the oxide vof carbon and hydrogen steam, iff the output in CH2() is not diminished and the. risl1 of forming alarge quantity of formic aci The formaldehyde produced, `mixed with the steam; is condensed in any suitable apparatus, for example in a column of cold water which thus enriches in formaldehyde as fast as the reaction takes place.

I may likewise obtain bythe action of these radiations photochemically on the same gas, an action of polymerizatlon with the formation of formose, this latter body being reduced by the excess of hydrogen which is uncombined (to which is added if necessary the desired amount of surplus hydrogen) in a way to give way to essences or oils.

In the case where the gas utilized contains methane I can obtain with the same appa- 'ratus a reaction of condensation between the methane and the formaldehyde, with productionv likewise of essences and oils.

Having described my invention what I claim as new and desire to secure by Lette Patent is:

1. Apparatus for the production of photochemical radiations of high activity comprising a high pressure inclosure, mercury filled electrode tubes having their upper extremities open, hollow tubes dipping in the mercury of said electrode tubes, the upper' ends of said hollow tubes being connected together to form a chamber constituting a burner, and means for circulating a cooling liuid at high pressure around said hollow tubes, the mervcury intermediate the high pressure inclosure i and said burner forming a seal whereby all variations in internal pressure/of the mercury vapor are transmitted-to the cooling iiuid and autoequilibration is established.

2. Apparatus for the production of photochemical radiationsof high activity com rising a high pressure inclosure, mercury lled electrode tubes having thei-r upper extremities open, hollow tubes of quartz dipping in the mercury of said electrode tubes, the upper. ends of saidhollowtubes being connected together to from a chamber constituting a burner, and means for'cireulating a cooling iuid at high pressurei around said hollow tubes, the mercury. intermediate the high pressure inclosure and said burner forming, a seal whereby all variations in internal pressure of the mercury vapor are transmitted' to the vcooling fluid and autoequilibration is established.

chemical radiations of high activity comprising a high pressureinclosure, mercury filled electrode-tubes having their upper eX- tremities open, hollow tubes dipping in the mercury of said electrode tubes, the upper ends of 'said hollow tubes being connected together to forma chamber constituting a burner, means for transmitting the radiations from the-high temperature arc formed to a.

point outside of' the apparatus and means for circulating a cooling iuid at h igh pressure around said hollow tubes, the mercury intermediate the high pressure inclosure and said burner forming a seal whereby all varia- 5 tions in internal pressure of the mercury vapor are transmitted to the cooling fluid and autoequilibration is established.

' x4. Apparatus for the production of photochemical radiations of high activity compris- 2 ing a high pressure inclosure, mercury filled o around said hollow tubes, the mercury intermediate the high-pressure inclosure and said burner forming a seal whereby all variations in internal pressure of the mercury vapor are transmitted to the cooling Huid and auto- .equilibration is established.

5. Apparatus for the production of photochemical radiations of high activity comprising a-high pressure inc'losure provided with an aperture, mercury filled electrode tubes having their upper extremities open, hollow tubes dipping in the mercury of said electrode tubes, the upper ends of said hollow tubes being connected together to form a chamber constituting a burner, said aperture provided with a lens for transmitting the radiations from the high temperature arc formed to a point outside of theapparats, a and means for circulating a cooling fluid at high' pressure around said hollow tubes, the v mercury intermediate the high pressure inclosure and said burner Jforming a seal-where*- by all variations in internal pressure of the mercury vapor are 'transmitted to the cooling fluid and autoequilibration isestablished.-

6'.` Apparatus for the production of photochemical -radiations of high activity comprising' a high pressureinclosure provided with an aperture, mercury filled electrode arc formed to a point outside of the apparatus, and means for circulating a cooling Huid at high pressure around said hollow tubes, the mercury intermediate the high pressure inclosure and said burner forming a seal whereby all variations in internal pressure of the mercury vapor are transmitted to the cooling fluid and autoequilibration is established. f

4In testimony whereof I have signed this specification.

HENRY SPINDLER.

4tubes having their upper extremities open,

hollow tubes of quartz dipping in the mercury of said electrode tubes, the upper ends of usaid hollow tubes being connected together to form a'c'h'amber constituting a burner, said aperture provided with a lens for transmit- 5 ting the radiations from the high temperature 

